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Tailoring residue-derived carbon materials for the removal of wastewater contaminants: adsorption and surface properties
Umeå University, Faculty of Science and Technology, Department of Chemistry.ORCID iD: 0000-0002-8890-835x
2019 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The availability of effective, low-cost wastewater treatment is necessary for increased water recycling and the prevention of environmental pollution on a global scale. Adsorption on activated carbons is commonly applied in wastewater treatment, but the high cost of conventional activated carbons limits the use of this technique. Several waste streams, such as the residues and by-products of food processing, agriculture and industrial processes, are currently inefficiently utilized and could be transformed into value-added carbon materials. Re-thinking how waste is utilized could reduce waste handling costs and increase resource efficiency, which would provide both economic and environmental benefits. Therefore, low-cost carbon materials prepared from renewable low-cost resources are an attractive alternative to decreasing the costs of wastewater treatment.

The research underlying this thesis investigated the potential of carbonized residue materials to remove environmentally relevant concentrations of organic and inorganic contaminants from wastewater. The research covered in this thesis included the carbonization of tomato- and olive press wastes, rise husks, horse manure, municipal wastewater sludge and bio- and fiber sludges from pulp and paper mills. The effect of carbonization temperature and starting material was studied in terms of surface properties and contaminant removal to gain knowledge on which surface features are beneficial for the removal of different contaminants. The extent to which different chemical activations of carbonized materials improve the contaminant removal was also studied.

The results demonstrate that carbonized materials are generally quite ineffective at removing organic compounds from water, which may be due to the low surface areas of these materials. Carbonization temperature was shown to alter the surface functionalities of the carbons, more specifically, high carbonization temperatures decreased oxygen-containing surface functionalities that benefitted the removal of most contaminants (which was most pronounced for Zn and trimethoprim). Further experiments investigated the role of the water matrix, and the results unexpectedly showed higher removal from a complex water matrix. Chemical activation improved removal efficiencies for all of the studied compounds, with the most pronounced effects observed for organic compounds. The activated carbons were able to completely remove fluconazole and trimethoprim from the landfill leachate water, and also showed high removal efficiensies (50-96%) of Cu and Zn. Furthermore, the results showed that adsorbate compounds may interact with the adsorbent surface in diverse ways, for example, via properties such as porosity and the presence of oxygen-containing functionalities or minerals. Also, adsorbate hydrophobicity (log Kow) affected the removal of organic compounds in some of the studied hydrochars. The research discussed in this thesis has highlighted that future studies should study the broad range of environmentally-relevant adsorbates through multi-component adsorption systems that include several complex water matrices.

Place, publisher, year, edition, pages
Umeå: Umeå universitet , 2019. , p. 69
Keywords [en]
Adsorption, hydrochar, HTC, chemical activation, wastewater, pharmaceuticals, metals, surface properties, biobased residues
National Category
Other Chemistry Topics
Identifiers
URN: urn:nbn:se:umu:diva-158507ISBN: 978-91-7855-071-5 (print)OAI: oai:DiVA.org:umu-158507DiVA, id: diva2:1307880
Public defence
2019-05-24, KB.E3.01 (Lilla Hörsalen), KBC-huset, Umeå, 09:00 (English)
Opponent
Supervisors
Available from: 2019-05-03 Created: 2019-04-29 Last updated: 2019-05-02Bibliographically approved
List of papers
1. Using carbonized low-cost materials for removal of chemicals of environmental concern from water
Open this publication in new window or tab >>Using carbonized low-cost materials for removal of chemicals of environmental concern from water
2018 (English)In: Environmental science and pollution research international, ISSN 0944-1344, E-ISSN 1614-7499, Vol. 25, no 16, p. 15793-15801Article in journal (Refereed) Published
Abstract [en]

Adsorption on low-cost biochars would increase the affordability and availability of water treatment in, for example, developing countries. The aim of this study was to identify the precursor materials and hydrochar surface properties that yield efficient removal of compounds of environmental concern (CEC). We determined the adsorption kinetics of a mixture containing ten CECs (octhilinone, triclosan, trimethoprim, sulfamethoxasole, ciprofloxacin, diclofenac, paracetamol, diphenhydramine, fluconazole, and bisphenol A) to hydrochars prepared from agricultural waste (including tomato- and olive-press wastes, rice husks, and horse manure). The surface characteristics of the hydrochars were evaluated via diffuse reflectance infrared spectroscopy (DRIFTS), X-ray photoelectron spectroscopy (XPS), and N2-adsorption. Kinetic adsorption tests revealed that removal efficiencies varied substantially among different materials. Similarly, surface analysis revealed differences among the studied hydrochars and the degree of changes that the materials undergo during carbonization. According to the DRIFTS data, compared with the least efficient adsorbent materials, the most efficient hydrochars underwent more substantial changes during carbonization.

Place, publisher, year, edition, pages
Springer, 2018
Keywords
Hydrochar, Adsorption, Hydrothermal carbonization, Agro-industrial residues, Organic chemicals, Low-cost adsorbents
National Category
Environmental Sciences
Identifiers
urn:nbn:se:umu:diva-150787 (URN)10.1007/s11356-018-1781-0 (DOI)000434051300046 ()29582326 (PubMedID)
Available from: 2018-08-16 Created: 2018-08-16 Last updated: 2019-04-29Bibliographically approved
2. Tailoring the functionality of waste materials using hydrothermal carbonization for water treatment applications
Open this publication in new window or tab >>Tailoring the functionality of waste materials using hydrothermal carbonization for water treatment applications
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

Purpose:

The material properties of carbons from hydrothermal carbonization (HTC), typically referred to as hydrochars, are crucial for hydrochar use in adsorption-related applications. More knowledge is needed on how HTC temperature is altering material properties of different wet low-cost materials and how it is affecting adsorption of contaminants. Studies systematically comparing different feedstocks and carbonization temperatures are needed, because comparisons between available studies are obstructed by the differences in reaction conditions and analysis techniques. 

Methods: In this study, hydrochars were prepared at 180℃, 220℃, and 260℃ from fiber sludge and biosludge from a paper mill, digested sewage sludge, and horse manure. Surface properties of the raw materials and chars were characterized and the adsorption capacity of methylene blue was studied. 

Results: The most substantial change, i.e., a decrease in the oxygen-functionalities of cellulose-rich materials (horse manure and fiber sludge), was caused by degradation of cellulose, while digested sludge types (biosludge and sewage sludge) seemed not to change substantially with the HTC temperature. Adsorption capacities varied between 9.0 and 68 mg g-1 char, being highest for biosludge treated at 220℃. Adsorption dropped drastically at the highest HTC temperature (260℃), which may be due to the decrease in oxygen-containing functionalities. Also substantial differences were seen between different feedstock materials. 

Conclusions: These results suggest that adsorption properties can be tailored both by selection of HTC temperature and feedstock.

Keywords
Hydrochar, surface properties, paper mill sludge, digested sludge, horse manure, adsorption
National Category
Other Chemistry Topics
Identifiers
urn:nbn:se:umu:diva-158502 (URN)
Available from: 2019-04-29 Created: 2019-04-29 Last updated: 2019-04-30
3. The water matrix influences the removal of organic and inorganic contaminants from landfill leachate by sludge and manure hydrochars
Open this publication in new window or tab >>The water matrix influences the removal of organic and inorganic contaminants from landfill leachate by sludge and manure hydrochars
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(English)Manuscript (preprint) (Other academic)
Abstract [en]

The removal of contaminants from water using low-cost adsorbents has been widely studied, yet studies employing a realistic water matrix are still lacking. This study investigated the removal of organic compounds (trimethoprim, fluconazole, and perfluorooctanoic acid (PFOA)) and metals (As, Zn, and Cu) from landfill leachate. Additionally, tests in pure water, humic acid and ion matrices were carried out to better understand how the water matrix affects adsorption. The hydrochars were produced from four feedstocks at three carbonization temperatures. The results show that the removal efficiencies for organic pollutants were low and metal removal by hydrochars was comparable to commercial activated carbon. The removal of all compounds from pure water was substantially lower. Tests with humic acid and ion-containing matrices could not fully explain the increased removal in the landfill leachate, which may be due to the combination of the water matrix and presence of soluble species from the hydrochars.

National Category
Other Chemistry Topics
Identifiers
urn:nbn:se:umu:diva-158504 (URN)
Available from: 2019-04-29 Created: 2019-04-29 Last updated: 2019-04-30
4. From waste to water treatment: Physicochemical and wastewater adsorption properties of activated hydrothermally carbonized waste materials
Open this publication in new window or tab >>From waste to water treatment: Physicochemical and wastewater adsorption properties of activated hydrothermally carbonized waste materials
(English)Manuscript (preprint) (Other academic)
Abstract [en]

Activated carbon forms an important step in the treatment of waste water in water treatment facilities. These facilities produce a range of underutilized sludge materials, which can be synthesized into activated carbon, reducing the amount of disposed sludge. Other waste materials high in organic matter, such as horse manure, are also ideal contenders for activated carbon upgrading. This study compares the hydrothermal carbonization followed by activation of sewage sludge and horse manure. Chemical activation was conducted using KOH and H3PO4, with physicochemical properties and adsorption of multiple contaminants being tested. Yield and inorganic content varied considerably, with KOH activated materials producing lower yields with higher inorganic content. A maximum surface area of 1363 m2g-1 and 343 m2g-1 was achieved for the horse manure and sewage sludge, respectively. Horse manure activated carbons displayed a high affinity for all adsorbates, other than arsenic, which was associated with high carbon content, carbon-oxygen functional groups and low mineral content.

National Category
Other Chemistry Topics
Identifiers
urn:nbn:se:umu:diva-158506 (URN)
Available from: 2019-04-29 Created: 2019-04-29 Last updated: 2019-04-30

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